First-principles prediction of high carrier mobility for ß-phase MX2N4 (M = Mo, W; X = Si, Ge) monolayers.

The recently synthesized monolayer MoSi2N4 (Science 2020, 369, 367) exhibits exceptional environmental stability, a moderate band gap, and excellent mechanical properties, presenting exciting opportunities for the exploration of two-dimensional (2D) MX2Z4 materials. However, the low carrier mobility of α-phase MoSi2N4 significantly limits its potential applications in field-effect transistor (FET) devices. In this study, we systematically investigate the structural stability, elastic properties, and carrier mobility of a novel family of ß-phase MX2N4 (M = Mo, W; X = Si, Ge) monolayers through first-principles calculations. Our findings reveal that these ß-phase MX2N4 monolayers demonstrate remarkable dynamic, thermal, and mechanical stability. Specifically, we identify the MoSi2N4, MoGe2N4, WSi2N4, and WGe2N4 monolayers as semiconductors with band gaps of 2.70 eV, 1.57 eV, 3.12 eV, and 1.93 eV, respectively, as calculated using the HSE06 functional. Moreover, the MX2N4 monolayers exhibit significant elastic anisotropy, characterized by high ideal tensile strengths and a critical tensile strain exceeding 25%. Notably, the WGe2N4 monolayer displays exceptional anisotropic in-plane charge transport, achieving mobility levels of up to 104 cm2V- 1S- 1, surpassing those of the α-phase MX2N4 monolayers. These novel ternary monolayer structures have the potential to broaden the 2D MX2Z4 material family and emerge as promising candidates for applications in field-effect transistors.

Intercalated Architecture of the Ca2A2Z5 Monolayer with High Electron Mobilities and High Power Conversion Efficiencies.

The exploration of novel two-dimensional (2D) materials with a direct band gap and high mobility has attracted huge attention due to their potential application in electronic and optoelectronic devices. Here, we propose a feasible way to construct multiatomic monolayer Ca2A2Z5 (A = Al and Ga and Z = S, Se, and Te) by first-principles calculations. Our results indicated that the energies of α1-phase Ca2A2Z5 are slightly lower than those of experimentally synthesized α3-phase-like Ca2A2Z5 monolayers with excellent structural stability. Moreover, the α1- and α3-phase Ca2A2Z5 monolayers possess not only direct band gaps but also high electron mobilities (up to ∼103 cm2 V-1 s-1), demonstrating an intriguing range of visible light absorption. Importantly, α1- and α3-phase Ca2Ga2Se5 monolayers are good donor materials, and the corresponding Ca2Ga2Se5/ZrSe2 type-II heterostructures exhibit desirable power conversion efficiencies of 22.4% and 22.9%, respectively. Our findings provide a feasible way to explore new 2D materials and offer several Ca2A2Z5 candidate monolayers for the application of high-performance solar cells.

High Performance Aqueous Zinc-Ion Batteries Developed by PANI Intercalation Strategy and Separator Engineering.

Aqueous zinc-ion batteries (ZIBs) have attracted burgeoning attention and emerged as prospective alternatives for scalable energy storage applications due to their unique merits such as high volumetric capacity, low cost, environmentally friendly, and reliable safety. Nevertheless, current ZIBs still suffer from some thorny issues, including low intrinsic electron conductivity, poor reversibility, zinc anode dendrites, and side reactions. Herein, conductive polyaniline (PANI) is intercalated as a pillar into the hydrated V2O5 (PAVO) to stabilize the structure of the cathode material. Meanwhile, graphene oxide (GO) was modified onto the glass fiber (GF) membrane through simple electrospinning and laser reduction methods to inhibit dendrite growth. As a result, the prepared cells present excellent electrochemical performance with enhanced specific capacity (362 mAh g-1 at 0.1 A g-1), significant rate capability (280 mAh g-1 at 10 A g-1), and admirable cycling stability (74% capacity retention after 4800 cycles at 5 A g-1). These findings provide key insights into the development of high-performance zinc-ion batteries.

Tuning charge transport by manipulating concentration dependent single-molecule absorption configurations.

Understanding and tuning charge transport in molecular junctions is pivotal for crafting molecular devices with tailored functionalities. Here, we report a novel approach to manipulate the absorption configuration within a 4,4'-bipyridine (4,4'-BPY) molecular junction, utilizing the scanning tunneling microscope break junction technique in a concentration-dependent manner. Single-molecule conductance measurements demonstrate that the molecular junctions exhibit a significant concentration dependence, with a transition from high conductance (HC) to low conductance (LC) states as the concentration decreases. Moreover, we identified an additional conductance state in the molecular junctions besides already known HC and LC states. Flicker noise analysis and theoretical calculations provided valuable insights into the underlying charge transport mechanisms and single-molecule absorption configurations concerning varying concentrations. These findings contribute to a fundamental comprehension of charge transport in concentration-dependent molecular junctions. Furthermore, they offer promising prospects for controlling single-molecule adsorption configurations, thereby paving the way for future molecular devices.

Ku-Band Mixers Based on Random-Oriented Carbon Nanotube Films.

Carbon nanotubes (CNTs) are a type of nanomaterial that have excellent electrical properties such as high carrier mobility, high saturation velocity, and small inherent capacitance, showing great promise in radio frequency (RF) applications. Decades of development have been made mainly on cut-off frequency and amplification; however, frequency conversion for RF transceivers, such as CNT-based mixers, has been rarely reported. In this work, based on randomly oriented carbon nanotube films, we focused on exploring the frequency conversion capability of CNT-based RF mixers. CNT-based RF transistors were designed and fabricated with a gate length of 50 nm and gate width of 100 µm to obtain nearly 30 mA of total current and 34 mS of transconductance. The Champion RF transistor has demonstrated cut-off frequencies of 78 GHz and 60 GHz for fT and fmax, respectively. CNT-based mixers achieve high conversion gain from -11.4 dB to -17.5 dB at 10 to 15 GHz in the X and Ku bands. Additionally, linearity is achieved with an input third intercept (IIP3) of 18 dBm. It is worth noting that the results from this work have no matching technology or tuning instrument assistance, which lay the foundations for the application of Ku band transceivers integrated with CNT amplifiers.

A near-infrared photodetector based on carbon nanotube transistors exhibits ultra-low dark current through field-modulated charge carrier transport.

Near-infrared photodetectors (NIR PDs) are devices that convert infrared light signals, which are widely used in military and civilian applications, into electrical signals. However, a common problem associated with PDs is a high dark current. Interestingly, gate voltage can regulate carrier migration in the channels. In this study, a PbS quantum dot heterojunction combined with a carbon nanotube (CNT) field effect transistor (FET) is designed and described. Significantly, this NIR PD achieves field-modulated carrier transport in a CNT transistor, in which the dark current is effectively regulated by the gate voltage. In this PD, an ultra-low dark current of 8 pA is obtained by gate voltage regulation. Moreover, the device shows a fast response speed of 6.5 ms and a high normalized detectivity of 4.75 × 1011 Jones at 0.085 W cm-2 power density and -0.2 V bias voltage. Overall, this work details a novel strategy for the fabrication of a PD with an ultra-low dark current based on a FET.

Aligned Carbon Nanotubes-Based Radiofrequency Transistors for Amplitude Amplification and Frequency Conversion at Millimeter Wave Band.

Aligned carbon nanotubes (ACNTs) have been considered as a promising candidate semiconductor with great potential in radiofrequency (RF) electronics due to their high carrier mobility/saturation velocity and small intrinsic capacitance. However, almost all of previously reported works focused on only the cutoff frequency, which is far from enough for practical RF application. In this work, given the speed advantage of ACNTs, we further explore amplitude amplification and frequency conversion capability of ACNTs based RF devices simultaneously, which are two basic functions in RF electronics. Considering there is no de-embedding process for amplification/conversion and reduction power loss, multifinger configuration RF transistors (still having current density around 1 mA/µm) were fabricated with cutoff frequency and maximum oscillation frequency exceeding 150 and 130 GHz, respectively. Based on dedicated ACNTs based RF FETs, we demonstrate almost 7 dB power gain (S21) with over 40 GHz 3-dB bandwidth for amplification and from -12.7 to -17 dB of conversion gain with over 25 dBm IIP3 (input third-order intercept point) of linearity for conversion simultaneously operating at 30 GHz in millimeter wave (mmWave) band both without any tuning instruments and matching technology assistance. The performance achieved here is the best among all the nanomaterials at the mmWave band.

Wafer-Scale Field-Effect Transistor-Type Sensor Using a Carbon Nanotube Film as a Channel for Ppb-Level Hydrogen Sulfide Detection.

Sulfur hexafluoride is widely used in power equipment because of its excellent insulation and arc extinguishing properties. However, severe damage to power equipment may be caused and a large-scale collapse of the power grid may occur when SF6 is decomposed into H2S, SOF2, and SO2F2. It is difficult to detect the SF6 concentration as it is a kind of inert gas. Generally, the trace gas decomposed in the early stage of SF6 is detected to achieve the function of early warning. Consequently, it is of great significance to realize the real-time detection of trace gases decomposed from SF6 for the early fault diagnosis of power equipment. In this work, a wafer-scale gate-sensing carbon-based FET gas sensor is fabricated on a four-inch carbon wafer for the detection of H2S, a decomposition product of SF6. The carbon nanotubes with semiconductor properties and the noble metal Pt are respectively used as a channel and a sensing gate of the FET-type gas sensor, and the channel transmission layer and the sensing gate layer each play an independent role and do not interfere with each other by introducing the gate dielectric layer Y2O3, giving full play to their respective advantages to forming an integrated sensor of gas detection and signal amplification. The detection limit of the as-prepared gate-sensing carbon-based FET gas sensor can reach 20 ppb, and its response deviation is not more than 3% for the different batches of gas sensors. This work provides a potentially useful solution for the industrial production of miniaturized and integrated gas sensors.

Dielectric modulation strategy of carbon nanotube field effect transistors based pressure sensor: towards precise monitoring of human pulse.

Continuous monitoring of arterial pulse has great significance for detecting the early onset of cardiovascular disease and assessing health status, while needs pressure sensors with high sensitivity and signal-to-noise ratio (SNR) to accurately capture more health information concealed in pulse waves. Field effect transistors (FETs) combined with the piezoelectric film is an ultrahigh sensitive pressure sensor category, especially when the FET works in the subthreshold regime, where the signal enhancement effect on the piezoelectric response is the most effective. However, controlling the work regime of FET needs extra external bias assistance which will interfere with the piezoelectric response signal and complicate the test system thus making the scheme difficult to implement. Here, we described a gate dielectric modulation strategy to match the subthreshold region of the FET with the piezoelectric output voltage without external gate bias, finally enhancing the sensitivity of the pressure sensor. A carbon nanotube field effect transistor and polyvinylidene fluoride (PVDF) together form the pressure sensor with a high sensitivity of 7 × 10-1kPa-1for a pressure range of 0.038-0.467 kPa and 6.86 × 10-2kPa-1for a pressure range of 0.467-15.5 kPa, SNR, and the ability to continuously monitor pulse in real-time. Additionally, the sensor enables high-resolution detection of weak pulse signals under large static pressure.

Tuning magnetocrystalline anisotropy by controlling the orbital electronic configuration of two-dimensional magnetic materials.

A suitable magnetic anisotropy energy (MAE) is a key factor for magnetic materials. However, an effective MAE control method has not yet been achieved. In this study, we propose a novel strategy to manipulate MAE by rearranging the d-orbitals of metal atoms with oxygen functionalized metallophthalocyanine (MPc) by first-principles calculations. By the dual regulation of electric field and atomic adsorption, we have achieved a substantial amplification of the single regulation method. The use of O atoms to modify the metallophthalocyanine (MPc) sheets effectively adjusts the orbital arrangement of the electronic configuration in the d-orbitals of the transition metal near the Fermi level, thereby modulating the MAE of the structure. More importantly, the electric field amplifies the effect of electric-field regulation by adjusting the distance between the O atom and metal atom. Our results demonstrate a new approach to modulating the MAE of two-dimensional magnetic films for practical application in information storage.

Novel three-dimensional TiO2 structure with a unique quasi-direct band gap for photocatalysts.

Motivated by fundamental interests and practical applications, three-dimensional (3D) photocatalysts are a fascinating area of research in clean energy. Based on first-principles calculations, we predicted three new 3D polymorphs of TiO2: δ-, ε-, and ζ-TiO2. Our results indicate that the band gaps of TiO2 decrease almost linearly with an increase in the coordination number of Ti. Moreover, δ-TiO2 and ζ-TiO2 are semiconductors, whereas ε-TiO2 is a metal, and the lowest energy of ζ-TiO2 is a quasi-direct band gap semiconductor with a distinctive band gap of 2.69 eV, calculated by the HSE06 level. In addition, the calculated imaginary part of the dielectric function indicates that the optical absorption edge is located in the visible light region, suggesting that the proposed ζ-TiO2 may be a good photocatalyst candidate. Importantly, ζ-TiO2 with the lowest energy is dynamically stable, and phase diagrams based on total energies at a specific pressure indicate that ζ-TiO2 can be synthesized from rutile TiO2 at high-pressure conditions.

Carbon Nanotube Field-Effect Transistor Biosensor with an Enlarged Gate Area for Ultra-Sensitive Detection of a Lung Cancer Biomarker.

Carcinoembryonic antigen (CEA) is a recognized biomarker for lung cancer and can be used for early detection. However, the clinical value of CEA is not fully realized due to the rigorous requirement for high-sensitivity and wide-range detection methods. Field-effect transistor (FET) biosensors, as one of the potentially powerful platforms, may detect CEA with a significantly higher sensitivity than conventional clinical testing equipment, while their sensitivity and detection range for CEA are far below the requirement for early detection. Here, we construct a floating gate FET biosensor to detect CEA based on a semiconducting carbon nanotube (CNT) film combined with an undulating yttrium oxide (Y2O3) dielectric layer as the biosensing interface. Utilizing an undulating biosensing interface, the proposed device showed a wider detection range and optimized sensitivity and detection limit, which benefited from an increase of probe-binding sites on the sensing interface and an increase of electric double-layer capacitance, respectively. The outcomes of analytical studies confirm that the undulating Y2O3 provided the desired biosensing surface for probe immobilization and performance optimization of a CNT-FET biosensor toward CEA including a wide detection range from 1 fg/mL to 1 ng/mL, good linearity, and high sensitivity of 72 ag/mL. More crucially, the sensing platform can function normally in the complicated environment of fetal bovine serum, indicating its great promise for early lung cancer screening.

Carbon Nanotube Transistor with Colloidal Quantum Dot Photosensitive Gate for Ultrahigh External Quantum Efficiency Photodetector.

PbS colloidal quantum dots (CQDs) are promising building block for developing the next-generation high-performance near-infrared (NIR) photodetector. However, due to the surface ligand isolation and surface defects, PbS CQDs usually suffer from low carrier mobility, which limits further optimization of PbS CQDs-based optoelectronic devices. Here, the combination of PbS CQD photodiode and carbon nanotube (CNT) film field-effect transistor (FET) achieves a transistorized NIR photodetector with a photosensitive gate. The photogenerated electrons are drifted to the dielectric surface by a negative gate electric field and built-in electric field, serving as an equivalent gate voltage to turn on the CNT FET, thus realizing the conversion of optical signals to electrical signals. The photodetector exhibits high performance, with a responsivity and detectivity of 41.9 A/W and 3.04 × 1011 Jones under 950 nm illumination, respectively. More importantly, the photodetector achieves an ultrahigh external quantum efficiency (EQE) of 5470% due to the CNT FET amplification function. Besides, the photodetector demonstrates a versatile photoresponse that allows for regulation of responsivity, detectivity, and EQE over a wide range through gate voltage control. The photodetector shows immense potential in NIR photodetection applications, and the distinctive structure of the optical module and electrical module separation also provides fresh thinking for the research and development of the next generation of optoelectronic devices.

Ultralow diffusion barrier induced by intercalation in layered N-based cathode materials for sodium-ion batteries.

Sodium-ion batteries (SIBs) have attracted huge attention due to not only the similar electrochemical properties to Lithium-ion batteries (LIBs) but also the abundant natural reserves of sodium. However, the high diffusion barrier has hindered its application. In this work, we have theoretically studied the relationship between the strain and the diffusion barrier/path of sodium ions in layered CrN2 by first-principles calculation. Our results show that the strain can not only effectively decrease the diffusion barrier but also change the sodium diffusion path, which can be realized by alkali metal intercalation. Moreover, the diffusion barrier is as low as 0.04 eV with the Cs atoms embedding in layered CrN2 (Cs1/16CrN2), suggesting an excellent candidate cathode for SIBs. In addition, the decrease of the barrier mainly originated from the fact that interlayer electronic coupling weakened with the increase of interlayer spacing. Our findings provide an effective way to enhance sodium diffusion performance, which is beneficial for the design of SIB electrode materials.

Optimization of the Mixed Gas Detection Method Based on Neural Network Algorithm.

Real-time mixed gas detection has attracted significant interest for being a key factor for applications of the electronic nose (E-nose). However, mixed gas detection still faces the challenge of long detection time and a large amount of training data. Therefore, in this work, we propose a feasible way to realize low-cost fast detection of mixed gases, which uses only the part response data of the adsorption process as the training set. Our results indicated that the proposed method significantly reduced the number of training sets and the prediction time of mixed gas. Moreover, it can achieve new concentration prediction of mixed gas using only the response data of the first 10 s, and the training set proportion can reduce to 60%. In addition, the convolutional neural network model can realize both the smaller training set but also the higher accuracy of mixed gas. Our findings provide an effective way to improve the detection efficiency and accuracy of E-noses for the experimental measurement.

New family of layered N-based cathode materials for sodium-ion batteries.

The cathode materials of sodium-ion batteries (SIBs) have received considerable attention not only because of their abundant natural reserves and chemical properties similar to those of lithium-ion batteries but also their great potential in energy storage and conversion technologies. However, their low capacity and high diffusion barrier remain unsolved problems. In this work, we systematically studied the theoretical capacity and sodium ion diffusion barrier in a new family of layered transition metal compounds, named MX2 (M = Ti, V, Cr, Mn, and Fe; X = C, N, and O), as the cathode materials of SIBs. The results indicate that all 2H-phase MX2 materials possess a high theoretical capacity of over 300 mA h g-1. Moreover, it is found that the 2H-phase CrN2 exhibits a desirable sodium ion diffusion barrier, indicating high mobility of sodium ions. In addition, the layered CrN2 has a remarkable voltage window (3.1-3.8 V) and outstanding electrochemical performance arising from the charge transfer between Na and N atoms, which is induced by the large electronegativity of nitrogen. Our research provides a promising candidate for application in SIB cathode materials in the future.

Atomic mechanism of lithium intercalation induced phase transition in layered MoS2.

The phase transition in layered MoS2 has attracted wide attention but the detailed phase transition process is still unclear. Here, the H → T' phase transition mechanism of single- and bilayer MoS2 induced by lithium intercalation has been systematically studied using first principles. The results indicated that the lithium intercalation can effectively reduce the sliding barrier of the S atom layer. Moreover, we demonstrated that the phase transition process in bilayer MoS2 is induced by S atom transition one by one instead of the collective behavior of the S atoms. Importantly, we found that the phase transition process in bilayer MoS2 consists of the formation, diffusion and recombination of S vacancies, and the phase transition originates from interlayer lithium defects. In addition, the lithium defects cannot induce phase transition in monolayer MoS2 due to the larger sliding barrier of the S atom.

High Anisotropic Optoelectronics in Monolayer Binary M8X12 (M = Mo, W; X = S, Se, Te).

Exploring high performance and excellent ambient stability in two-dimensional (2D) monolayer photoelectric materials is motivated by not only practical applications but also scientific interest. Here, a new 2D monolayer W8Se12 structure is synthesized via in situ electron-beam irradiation on 2D WSe2. Moreover, we systematically studied the photoelectric properties of the class of monolayer M8X12 (M = Mo, W; X = S, Se, and Te) materials by first principles. The results indicated that Mo8S12, Mo8Se12, W8S12, and W8Se12 monolayers possess desirable direct band gaps and remarkable anisotropic optical absorption in visible light, while Mo8Te12 and W8Te12 monolayers are metals. Impressively, the monolayer W8Se12 can result in a direct-indirect-metal transition under uniaxial strain. In addition, they show high anisotropic carrier mobilities (up to 104 cm2 V-1 s-1), significantly over those of transition-metal dichalcogenides. These new binary monolayer M8X12 structures can effectively broaden the 2D material family and may provide four potential candidates in photoelectric applications.

The Characteristic of Fe as a ß-Ti Stabilizer in Ti Alloys.

It is well known that adding elements, especially ß-Ti stabilizers, are holding a significant effect on titanium alloy strength due to the solution and precipitate strengthening mechanisms. In order to reveal the Fe strengthening mechanism in titanium, this study investigate the effect of Fe on the stability of ß-Ti and the phase transition between α, ß and ω phase with first-principle calculations. According to our study, Fe is a strong ß-Ti phase stabilizer could owe to the 3d orbital into eg and t2g states which results in strong hybridization between Fe-d orbital and Ti-d orbital. The phase transition from ω to ß or from α to ß becomes easier for Fe-doped Ti compared to pure titanium. Based on our results, it is found that one added Fe atom can lead the phase transition (ω → ß) of at least nine titanium atoms, which further proves that Fe has a strong stabilizing effect on ß-Ti phase. This result provides a solid guide for the future design of high-strength titanium with the addition of Fe.

Carbon Nanotube-Based Field-Effect Transistor-Type Sensor with a Sensing Gate for Ppb-Level Formaldehyde Detection.

The detection of harmful trace gases, such as formaldehyde (HCHO), is a technical challenge in the current gas sensor field. The weak electrical signal caused by trace amounts of gases is difficult to be detected and susceptible to other gases. Based on the amplification effect of a field-effect transistor (FET), a carbon-based FET-type gas sensor with a gas-sensing gate is proposed for HCHO detection at the ppb level. Semiconducting carbon nanotubes (s-CNTs) and a catalytic metal are chosen as channel and gate materials, respectively, for the FET-type gas sensor, which makes full use of the respective advantages of the channel transport layer and the sensitive gate layer. The as-prepared carbon-based FET-type gas sensor exhibits a low detection limit toward HCHO up to 20 ppb under room temperature (RT), which can be improved to 10 ppb by a further heating strategy. It also exhibits a remarkable elevated recovery rate from 80 to 97% with almost no baseline drift (2%) compared to the RT condition, revealing excellent reproducibility, stability, and recovery. The role of sensitive function in the FET-type gas sensor is performed by means of an independent gas-sensing gate, that is, the independence of the sensitive gate and the electron transmission channel is the main reason for its high sensitivity detection. We hope our work can provide an instructive approach for designing high-performance formaldehyde sensor chips with on-chip integration potential.